arXiv subjects

Luis M. Liz-Marzán

Publications and source records attributed to Luis M. Liz-Marzán.

11 recordsLinked to original sources

arXiv2026

Continuous three-dimensional imaging of nanoscale dynamics by in situ electron tomography

Visualizing nanoscale transformations in three dimensions (3D) is essential for understanding materials evolution under operating conditions, yet dynamic electron tomography remains limited by slow tilt series acquisition and by reconstruction methods that assume static specimens. These constraints prevent continuous 3D imaging of evolving structures and require electron doses that can alter the specimens and their dynamics. Here, we demonstrate a framework for dynamic electron tomography that combines continuous tilting with a self-supervised deep-learning reconstruction strategy. Our approach incorporates the temporal aspect into the electron tomography reconstruction process to recover 3D volumes at arbitrary time points from a single tilt series. We validate the method using simulations and demonstrate its merit in experimental studies of heat-induced transformations, including morphological evolution of Au nanostars and alloying in Au@Ag nanocubes. Our results establish a practical framework for dynamic, dose-efficient electron tomography, enabling in situ 3D investigation of nanomaterial transformations as well as the characterization of beam-sensitive structures.

cond-mat.mtrl-sci↗

arXiv2025

Machine Learning Integrated Near-Infrared Surface-Enhanced Raman Spectroscopy for Accurate Strain-Level Virus Identification

Strain-level identification of viruses is critical for effective public health responses to potential outbreaks, yet current diagnostic methods often lack the necessary speed or sensitivity. Surface-enhanced Raman spectroscopy (SERS) offers great potential for fast and precise virus clarification through unique vibrational fingerprints of biological components. However, existing protocols typically operate outside of the tissue's transparent near-infrared (NIR) window, and are further limited by the intrinsic complexity of clinical viral samples, which complicates spectral analysis and recognition. Here, we report an artificial intelligence (AI)-empowered NIR-SERS platform that integrates machine learning with a rationally designed hybrid substrate: gold nanostars (AuNSt) coupled with gold-coated carbon nanotube arrays (AuCNT). This architecture generates highly localized plasmonic hot spots resonant tuned to NIR excitation, as confirmed by electron energy-loss spectroscopy (EELS), enabling effective signal amplification from viral components. Our system and protocols provide accurate classification of respiratory viruses, including influenza viruses and coronaviruses, not only at the type and subtype levels, but also the more challenging strain level. This approach overcomes the plasmonic mismatch in conventional SERS and the lack of generalizability in AI-driven diagnostics. It shows promise for enhancing rapid virus detection and identification of novel strains and outbreak response capabilities, thus potentially addressing critical challenges in global public health preparedness.

physics.chem-ph↗

arXiv2025

Penta-twinned gold nanoparticles under pressure: a comprehensive study

We report on the high-pressure optical and mechanical properties of penta-twinned gold nanoparticles (PT-AuNPs) of different geometries: decahedra, rods and bipyramids. Our results show that, unlike single-crystal (SC-AuNPs), PT-AuNPs preserve both their non-cubic crystal structures and their overall morphology up to 30 GPa. This structural integrity under compression is related to an enhanced mechanical resilience of PT-AuNPs, despite exhibiting bulk moduli comparable to those of SC-AuNPs. Notwithstanding, comparable pressure-induced localized surface plasmon resonance redshifts - for all nanoparticle geometries - were observed. Our analysis indicates that these shifts are primarily caused by changes in the refractive index of the surrounding medium, with electron density compression playing a minor role, contrasting with the behavior in SC-AuNPs, where electron density compression has a greater influence.

cond-mat.mtrl-sci↗

arXiv2025

Transformable Plasmonic Helix with Swinging Gold Nanoparticles

Control over multiple optical elements that can be dynamically rearranged to yield substantial three-dimensional structural transformations is of great importance to realize reconfigurable plasmonic nanoarchitectures with sensitive and distinct optical feedback. In this work, we demonstrate a transformable plasmonic helix system, in which multiple gold nanoparticles (AuNPs) can be directly transported by DNA swingarms to target positions without undergoing consecutive stepwise movements. The swingarms allow for programmable AuNP translocations in large leaps within plasmonic nanoarchitectures, giving rise to tailored circular dichroism spectra. Our work provides an instructive bottom-up solution to building complex dynamic plasmonic systems, which can exhibit prominent optical responses through cooperative rearrangements of the constituent optical elements with high fidelity and programmability.

physics.bio-ph↗

arXiv2024

Origin of the rich polymorphism of gold in penta-twinned nanoparticles

We report on the crystallographic structure of penta-twinned gold nanoparticles. Although gold typically exhibits a face-centered cubic (fcc) lattice, other phases have been reported in some nanoscale systems. We show that the crystallographic system and the lattice parameters of the gold unit cell strongly depend on the nanoparticle geometry, for a wide size range. Specifically, we show that decahedra exhibit a body-centered tetragonal structure (I4/mmm), whereas rods and bipyramids exhibit a body-centered orthorhombic structure (Immm). These changes in the crystallographic structure are explained by the elastic lattice distortions required to close the mismatch gap in penta-twinned nanoparticles, with respect to fcc single-crystal gold nanoparticles. The effects of nanoparticle shape and size on the surface pressure and the subsequent distortions are additionally discussed.

cond-mat.mtrl-sci↗

arXiv2023

Liquid phase fast electron tomography unravels the true 3D structure of colloidal assemblies

Electron tomography has become a commonly used tool to investigate the three-dimensional (3D) structure of nanomaterials, including colloidal nanoparticle assemblies. However, electron microscopy is typically carried out under high vacuum conditions. Therefore, pre-treatment sample preparation is needed for assemblies obtained by (wet) colloid chemistry methods, including solvent evaporation and deposition on a solid TEM support. As a result of this procedure, changes are consistently imposed on the actual nanoparticle organization. Therefore, we propose herein the application of electron tomography of nanoparticle assemblies while in their original colloidal liquid environment. To address the challenges related to electron tomography in liquid, we devised a method that combines fast data acquisition in a commercial liquid-TEM cell, with a dedicated alignment and reconstruction workflow. We present the application of this method to two different systems, which exemplify the difference between conventional and liquid tomography, depending on the nature of the protecting ligands. 3D reconstructions of assemblies comprising polystyrene-capped Au nanoparticles encapsulated in polymeric shells revealed less compact and more distorted configurations for experiments performed in a liquid medium compared to their dried counterparts. On the other hand, quantitative analysis of the surface-to-surface distance of self-assembled Au nanorods in water agrees with previously reported dimensions of the ligand layers surrounding the nanorods, which are in much closer contact when in similar but dried assemblies. This study, therefore, emphasizes the importance of developing high-resolution characterization tools that preserve the native environment of colloidal nanostructures.

cond-mat.soft↗

arXiv2023

Anti-Stokes Photoluminescence in Monolayer WSe$_2$ Activated by Plasmonic Cavities through Resonant Excitation of Dark Excitons

Anti-Stokes photoluminescence (PL) is light emission at a higher photon energy than the excitation, with applications in optical cooling, bioimaging, lasing, and quantum optics. Here, we show how plasmonic nano-cavities activate anti-Stokes PL in WSe$_2$ monolayers through resonant excitation of a dark exciton. The tightly confined plasmonic fields excite the out-of-plane transition dipole of the dark exciton, leading to light emission from the bright exciton at higher energy. Through statistical measurements on hundreds of plasmonic cavities, we show that coupling to the dark exciton is key to achieving a near hundred-fold enhancement of the upconverted PL intensity. This is further corroborated by experiments in which the laser excitation wavelength is tuned across the dark exciton. Finally, we show that an asymmetric nanoparticle shape and precise geometry are key for consistent activation of the dark exciton and efficient PL upconversion. Our work introduces a new excitation channel for anti-Stokes PL in WSe$_2$ and paves the way for large-area substrates providing optical cooling, anti-Stokes lasing, and radiative engineering of excitons.

cond-mat.mes-hall↗

arXiv2022

Quantification of the helical morphology of chiral Au nanorods

Chirality in inorganic nanoparticles and nanostructures has gained increasing scientific interest, because of the possibility to tune their ability to interact differently with left- and right-handed circularly polarized light. In some cases, the optical activity is hypothesized to originate from a chiral morphology of the nanomaterial. However, quantifying the degree of chirality in objects with sizes of tens of nanometers is far from straightforward. Electron tomography offers the possibility to faithfully retrieve the three-dimensional morphology of nanomaterials, but only a qualitative interpretation of the morphology of chiral nanoparticles has been possible so far. We introduce herein a methodology that enables us to quantify the helicity of complex chiral nanomaterials, based on the geometrical properties of a helix. We demonstrate that an analysis at the single particle level can provide significant insights into the origin of chiroptical properties.

cond-mat.mes-hall↗

arXiv2020

Can Copper Nanostructures Sustain High-Quality Plasmons?

Silver is considered to be the king among plasmonic materials because it features low inelastic absorption in the visible and infrared (vis-IR) spectral regions compared to other metals. In contrast, copper is commonly regarded as being too lossy for plasmonic applications. Here, we experimentally demonstrate vis-IR plasmons in long copper nanowires (NWs) with quality factors that exceed a value of 60, as determined by spatially resolved, high-resolution electron energy-loss spectroscopy (EELS) measurements. We explain this counterintuitive result by the fact that plasmons in these metal wires have most of their electromagnetic energy outside the metal, and thus, they are less sensitive to inelastic losses in the material. We present an extensive set of data acquired on long silver and copper NWs of varying diameters supporting this conclusion and further allowing us to understand the relative roles played by radiative and nonradiative losses in plasmons that span a wide range of energies down to $<20\,$meV. At such small plasmon energies, thermal population of these modes becomes significant enough to enable the observation of electron energy gains associated with plasmon absorption events. Our results support the use of copper as an attractive cheap and abundant material platform for high quality plasmons in elongated nanostructures.

cond-mat.mtrl-sci↗

arXiv2014

Monitoring Galvanic Replacement Through Three-Dimensional Morphological and Chemical Mapping

Galvanic replacement reactions on metal nanoparticles are often used for the preparation of hollow nanostructures with tunable porosity and chemical composition, leading to tailored optical and catalytic properties. However, the precise interplay between the three-dimensional (3D) morphology and chemical composition of nanostructures during Galvanic replacement is not always well understood as the 3D chemical imaging of nanoscale materials is still challenging. It is especially far from straightforward to obtain detailed information from the inside of hollow nanostructures using electron microscopy techniques such as SEM or TEM. We demonstrate here that a combination of state-of-the-art EDX mapping with electron tomography results in the unambiguous determination of both morphology transformation and elemental composition of nanostructures in 3D, during Galvanic replacement of Ag nanocubes. This work provides direct and unambiguous experimental evidence leading to new insights in the understanding of the galvanic replacement reaction. In addition, the powerful approach presented here can be applied to a wide range of nanoscale transformation processes, which will undoubtedly guide the development of novel nanostructures.

cond-mat.mtrl-sci↗

arXiv2014

Self-organisation of highly symmetric nanoassemblies: a matter of competition

The properties and applications of metallic nanoparticles are inseparably connected not only to their detailed morphology and composition, but also to their structural configuration and mutual interactions. As a result, the assemblies often have superior properties as compared to individual nanoparticles. Although it has been reported that nanoparticles can form highly symmetric clusters, if the configuration can be predicted as a function of the synthesis parameters, more targeted and accurate synthesis will be possible. We present here a theoretical model that accurately predicts the structure and configuration of self-assembled gold nanoclusters. The validity of the model is verified using quantitative experimental data extracted from electron tomography 3D reconstructions of different assemblies. The present theoretical model is generic and can in principle be used for different types of nanoparticles, providing a very wide window of potential applications.

cond-mat.mes-hall↗